Supertough Lignin Hydrogels with Multienergy Dissipative Structures and Ultrahigh Antioxidative Activities

Hydrogels derived from lignin are typically weak and contain only a small amount of lignin, which limits their broad application prospects. In the present work, a novel lignin/poly(N,N-dimethylacrylamide) (PDMA) hydrogel with a high lignin content, superb toughness, and ultrahigh antioxidative performance is constructed by employing a facile dissolve–dry–swell solvent exchange method. Through this process, lignin and PDMA are self-assembled into a multienergy dissipative structure containing rigid lignin-rich domains. Precisely, the PDMA chains both interpenetrated inside and adhered on the surface of these domains through hydrophobic associations. This structure enables the lignin hydrogels to dissipate energy efficiently during the fracture process. At an optimized ultrahigh lignin content of 58% (dry weight basis), the prepared lignin hydrogel exhibited remarkable mechanical properties, such as a high elastic modulus (2.5 MPa), tensile strength (2.5 MPa), and super tensile strain (11.3), and an extremely high fracture energy above 16 000 J m–2. In addition, the tough lignin hydrogel exhibited a commendable antioxidant property and nontoxicity. All these advantageous properties provide the lignin/PDMA hydrogels with the potential for use in biomedical materials applications.